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[ subject:"Chemistry, Physical." ]
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Ultrafast infrared studies of comple...
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University of California, Berkeley.
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Ultrafast infrared studies of complex ligand rearrangements in solution.
紀錄類型:
書目-語言資料,印刷品 : Monograph/item
正題名/作者:
Ultrafast infrared studies of complex ligand rearrangements in solution./
作者:
Payne, Christine K.
面頁冊數:
127 p.
附註:
Chair: Charles B. Harris.
Contained By:
Dissertation Abstracts International64-09B.
標題:
Chemistry, Physical. -
電子資源:
http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3105337
ISBN:
9780496529049
Ultrafast infrared studies of complex ligand rearrangements in solution.
Payne, Christine K.
Ultrafast infrared studies of complex ligand rearrangements in solution.
- 127 p.
Chair: Charles B. Harris.
Thesis (Ph.D.)--University of California, Berkeley, 2003.
The complete description of a chemical reaction in solution depends upon an understanding of the reactive molecule as well as its interactions with the surrounding solvent molecules. Using ultrafast infrared spectroscopy it is possible to observe both the solute-solvent interactions and the rearrangement steps which determine the overall course of a chemical reaction. The topics addressed in these studies focus on reaction mechanisms which require the rearrangement of complex ligands and the spectroscopic techniques necessary for the determination of these mechanisms.
ISBN: 9780496529049Subjects--Topical Terms:
560527
Chemistry, Physical.
Ultrafast infrared studies of complex ligand rearrangements in solution.
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Source: Dissertation Abstracts International, Volume: 64-09, Section: B, page: 4376.
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Thesis (Ph.D.)--University of California, Berkeley, 2003.
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The complete description of a chemical reaction in solution depends upon an understanding of the reactive molecule as well as its interactions with the surrounding solvent molecules. Using ultrafast infrared spectroscopy it is possible to observe both the solute-solvent interactions and the rearrangement steps which determine the overall course of a chemical reaction. The topics addressed in these studies focus on reaction mechanisms which require the rearrangement of complex ligands and the spectroscopic techniques necessary for the determination of these mechanisms.
520
$a
Ligand rearrangement is studied by considering two different reaction mechanisms for which the rearrangement of a complex ligand constitutes the most important step of the reaction. The first system concerns the rearrangement of a cyclopentadienyl ring as the response of an organometallic complex to a loss of electron density. This mechanism, commonly referred to as "ring slip", is frequently cited to explain reaction mechanisms. However, the ring slipped intermediate is too short-lived to be observed using conventional methods. Using a combination of ultrafast infrared spectroscopy and electronic structure calculations it has been shown that the intermediate exists, but does not form an eighteen-electron intermediate as suggested by traditional molecular orbital models.
520
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The second example examines the initial steps of alkyne polymerization. Group 6 (Cr, Mo, W) pentacarbonyl species are generated photolytically and used to catalyze the polymerization of unsaturated hydrocarbons through a series of coordination and rearrangement steps. Observing this reaction on the femto- to millisecond timescale indicates that the initial coordination of an alkyne solvent molecule to the metal center results in a stable intermediate that does not rearrange to form the polymer precursor. This suggests that polymerization requires the dissociation of additional carbonyl ligands before rearrangement can occur.
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Overall, this research demonstrates the importance of examining reaction dynamics on the ultrafast timescale. In the case of both ring slip and alkyne polymerization, early time dynamics have been invaluable in understanding the exact reaction mechanisms which show important differences from previously accepted models.
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http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=3105337
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